Metal-organic frameworks (MOFs) functionalized via Ir(I) cyclometalation are shown to be effective as heterogeneous catalysts for the allylic N-alkylation of various amines. The MOF catalysts are one of the first and most effective MOF-based heterogeneous organometallic catalysts for the direct formation of C-N bonds. In addition, these MOFs represent a rare, stable and reusable, class of reactive Ir catalysts.